Schottky Defects Suppress Nonradiative Recombination in CH3NH3PbI3 through Charge Localization

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters Pub Date : 2024-12-23 DOI:10.1021/acs.jpclett.4c03313

Lu Qiao, Andrey S. Vasenko, Evgueni V. Chulkov, Run Long

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Abstract

Hybrid lead halide perovskites are promising materials for photovoltaic applications due to their exceptional optoelectronic properties. Here, we investigate the impact of Schottky defects─specifically PbI₂(V_PbI₂) and CH₃NH₃I (V_MAI) vacancies─on nonradiative recombination in CH₃NH₃PbI₃ using time-dependent density functional theory and nonadiabatic (NA) molecular dynamics. Our results reveal that Schottky defects do not alter the fundamental bandgap or introduce trap states but instead distort the surrounding lattice, localizing the hole distribution. This reduces the spatial overlap of electron and hole wave functions, weakening NA coupling and increasing intensitieis of high-intensity phonon modes that accelerate dephasing. Consequently, nonradiative recombination lifetimes extend to 2.1 and 2.6 ns for V_PbI₂ and V_MAI, respectively─over double that of pristine CH₃NH₃PbI₃. This work demonstrates the potential of Schottky defects to enhance perovskite solar cell performance by suppressing nonradiative recombination.

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肖特基缺陷通过电荷局域化抑制CH3NH3PbI3的非辐射重组

杂化卤化铅钙钛矿具有优异的光电性能，是一种很有前途的光伏材料。本文利用时变密度泛函理论和非绝热（NA）分子动力学研究了肖特基缺陷──特别是PbI2（VPbI2）和CH3NH3I （VMAI）空位──对CH3NH3PbI3非辐射重组的影响。我们的研究结果表明，肖特基缺陷不会改变基本带隙或引入陷阱态，而是扭曲周围的晶格，使空穴分布局部化。这减少了电子和空穴波函数的空间重叠，减弱了NA耦合，增加了加速消相的高强度声子模式的强度。因此，VPbI2和VMAI的非辐射重组寿命分别延长至2.1和2.6 ns，是原始CH3NH3PbI3的两倍多。这项工作证明了肖特基缺陷通过抑制非辐射复合来提高钙钛矿太阳能电池性能的潜力。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY

CiteScore

9.60

自引率

7.00%

发文量

1519

审稿时长

1.6 months

期刊介绍： The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.